Three-Dimensional Tracking of Interfacial Hopping Diffusion

Wang, Dapeng; Wu, Haichao; Schwartz, Daniel K.

doi:10.1103/physrevlett.119.268001

Three-Dimensional Tracking of Interfacial Hopping Diffusion

Journal Article · Fri Dec 29 00:00:00 EST 2017 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.119.268001· OSTI ID:1541263

Wang, Dapeng ^[1]; Wu, Haichao ^[2]; Schwartz, Daniel K. ^[2]

Chinese Academy of Sciences (CAS), Changchun (China). State Key Lab. of Polymer Physics and Chemistry. Changchun Inst. of Applied Chemistry; Univ. of Colorado, Boulder, CO (United States). Dept. of Chemical and Biological Engineering; DOE/OSTI
Univ. of Colorado, Boulder, CO (United States). Dept. of Chemical and Biological Engineering

Theoretical predictions have suggested that molecular motion at interfaces—which influences processes including heterogeneous catalysis, (bio)chemical sensing, lubrication and adhesion, and nanomaterial self-assembly—may be dominated by hypothetical “hops” through the adjacent liquid phase, where a diffusing molecule readsorbs after a given hop according to a probabilistic “sticking coefficient.” Here, we use three-dimensional (3D) single-molecule tracking to explicitly visualize this process for human serum albumin at solid-liquid interfaces that exert varying electrostatic interactions on the biomacromolecule. Following desorption from the interface, a molecule experiences multiple unproductive surface encounters before readsorption. An average of approximately seven surface collisions is required for the repulsive surfaces, decreasing to approximately two and a half for surfaces that are more attractive. The hops themselves are also influenced by long-range interactions, with increased electrostatic repulsion causing hops of longer duration and distance. These findings explicitly demonstrate that interfacial diffusion is dominated by biased 3D Brownian motion involving bulk-surface coupling and that it can be controlled by influencing short- and long-range adsorbate-surface interactions.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Colorado, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001854

OSTI ID:: 1541263

Alternate ID(s):: OSTI ID: 1416445

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 26 Vol. 119; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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